PNNL

Abstract

We investigated the effects of water saturation and formation of secondary precipitates on transport of Sr and Cs through sand columns under unsaturated water flow. A series of column experiments was run at effective water saturations ranging from 0.2 to 1.0 under steady-state flow using columns filled with quartz sand. The solution phase was either 0.1 M NaNO3 or a simulated tank waste leachate (STWL), mimicking the leaks of tank wastes at the Hanford Site, Washington, USA. In STWL, the mobility of Sr was significantly reduced as the water saturation decreased, because Sr was incorporated into or sorbed to neo-formed secondary precipitates. In contrast, the transport of Cs in STWL was similar to that of a nonreactive tracer. In 0.1 M NaNO3, Sr moved like a conservative tracer, showing no retardation, whereas Cs was retarded relative to Sr. The flow regime for the 0.1 M NaNO3 columns under all water saturations could be described with the equilibrium convection-dispersion equation (CDE). However, for STWL, the Sr and Cs breakthrough curves indicated the presence of non-equilibria under unsaturated flow conditions. Such non-equilibrium conditions, caused by physical and chemical processes can reduce the mobility of radionuclides at the Hanford vadose zone.